ZnO nanorod array films grown on fluorine-doped tin oxide glass substrates were homogeneously coated with visible light responsive Cu₂SnS₃ nanoparticles through a controllable one-step electrodeposition process. The coating of Cu₂SnS₃ nanoparticles expanded light utilization from the UV to visible region and facilitated charge generation, separation and transportation, thus leading to significantly enhanced photoelectrochemical and photocatalytic performance. The ZnO/Cu₂SnS₃ nanorod array films with a deposition time of 90 s had the highest apparent rate constant (3.87 × 10⁻² min⁻¹) and photocurrent density (0.46 mA cm⁻²), which were 2.86 and 23.00 times that of the pure ZnO, respectively. The ZnO/Cu₂SnS₃ nanorod array films were proven to be an advanced structure for photoelectrochemical and recyclable photocatalytic applications due to the maintenance of the optimized Cu₂SnS₃ nanoparticle coating and array nanostructure.